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Title: Polarity-driven oxygen vacancy formation in ultrathin LaNiO 3 films on SrTiO 3

Abstract

Oxide heterostructures offer a pathway to control emergent phases in complex oxides, but their creation often leads to boundaries that have a polar discontinuity. In order to fabricate atomic-scale arrangements of dissimilar materials, we need a clear understanding of the pathways by which materials resolve polarity issues. By examining the real-time lattice structure in-situ during growth for the case of polar LaNiO3 synthesized on non-polar SrTiO3 (001), we demonstrate how films in ultra-thin limit form as LaNiO2.5 and then evolve into LaNiO3 as the thickness increases. Theory explains how the polar energetics drives the formation of oxygen vacancies and the stability of these phases with thickness and structure.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [6];  [2];  [4];  [6]
+ Show Author Affiliations
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  2. Univ. of Wisconsin, Madison, WI (United States). Dept. of Materials Science and Engineering
  3. Korea Atomic Energy Research Inst., Daejeon (Republic of Korea). Neutron Science Division
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  5. Univ. of Illinois, Urbana-Champaign, IL (United States). Materials Research Lab., Dept. of Physics
  6. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  7. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering; Northwestern Univ., Evanston, IL (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE
OSTI Identifier:
1425266
Alternate Identifier(s):
OSTI ID: 1400007
Grant/Contract Number:  
AC02-06CH11357; DMR-1121288; ACI-1053575
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 5; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Tung, I-Cheng, Luo, Guangfu, Lee, June Hyuk, Chang, Seo Hyoung, Moyer, Jarrett, Hong, Hawoong, Bedzyk, Michael J., Zhou, Hua, Morgan, Dane, Fong, Dillon D., and Freeland, John W. Polarity-driven oxygen vacancy formation in ultrathin LaNiO3 films on SrTiO3. United States: N. p., 2017. Web. doi:10.1103/physrevmaterials.1.053404.
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Tung, I-Cheng, Luo, Guangfu, Lee, June Hyuk, Chang, Seo Hyoung, Moyer, Jarrett, Hong, Hawoong, Bedzyk, Michael J., Zhou, Hua, Morgan, Dane, Fong, Dillon D., & Freeland, John W. Polarity-driven oxygen vacancy formation in ultrathin LaNiO3 films on SrTiO3. United States. https://doi.org/10.1103/physrevmaterials.1.053404
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Tung, I-Cheng, Luo, Guangfu, Lee, June Hyuk, Chang, Seo Hyoung, Moyer, Jarrett, Hong, Hawoong, Bedzyk, Michael J., Zhou, Hua, Morgan, Dane, Fong, Dillon D., and Freeland, John W. Wed . "Polarity-driven oxygen vacancy formation in ultrathin LaNiO3 films on SrTiO3". United States. https://doi.org/10.1103/physrevmaterials.1.053404. https://www.osti.gov/servlets/purl/1425266.
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@article{osti_1425266,
title = {Polarity-driven oxygen vacancy formation in ultrathin LaNiO3 films on SrTiO3},
author = {Tung, I-Cheng and Luo, Guangfu and Lee, June Hyuk and Chang, Seo Hyoung and Moyer, Jarrett and Hong, Hawoong and Bedzyk, Michael J. and Zhou, Hua and Morgan, Dane and Fong, Dillon D. and Freeland, John W.},
abstractNote = {Oxide heterostructures offer a pathway to control emergent phases in complex oxides, but their creation often leads to boundaries that have a polar discontinuity. In order to fabricate atomic-scale arrangements of dissimilar materials, we need a clear understanding of the pathways by which materials resolve polarity issues. By examining the real-time lattice structure in-situ during growth for the case of polar LaNiO3 synthesized on non-polar SrTiO3 (001), we demonstrate how films in ultra-thin limit form as LaNiO2.5 and then evolve into LaNiO3 as the thickness increases. Theory explains how the polar energetics drives the formation of oxygen vacancies and the stability of these phases with thickness and structure.},
doi = {10.1103/physrevmaterials.1.053404},
journal = {Physical Review Materials},
number = 5,
volume = 1,
place = {United States},
year = {Wed Oct 18 00:00:00 EDT 2017},
month = {Wed Oct 18 00:00:00 EDT 2017}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1103/physrevmaterials.1.053404
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Cited by: 25 works
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Figures / Tables:

Fig. 1 Fig. 1: (a) X-ray scattering from a series of LaNiO3 films with varying thickness measured immediately following the growth of the final layer under growth conditions and for the 11 u.c. (final) film structure measured immediately following the growth of 5th u.c. Solid lines are a fit to the datamore » discuss in the text. (b) Temperature dependence from 2–350 K of film resistivity showing that 11 u.c. is metallic as expected but 6 and 4 u.c. are insulating. (c) X-ray absorption at the Ni L2 edge was used to determine the sample valence. The inset shows the plot of the sample valence showing the variation from Ni2+ when the samples are very thin to the expected bulk Ni3+ value by 11 u.c.« less
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    Works referencing / citing this record:

    Carrier localization in perovskite nickelates from oxygen vacancies
    journal, October 2019

    • Kotiuga, Michele; Zhang, Zhen; Li, Jiarui
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 44
    • DOI: 10.1073/pnas.1910490116

    High-density electron doping of SmNiO 3 from first principles
    journal, November 2019

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